化学
化学反应
水溶液
硝基甲烷
双水相体系
合理化(经济学)
化学动力学
反应速率
动力学
环境化学
有机化学
催化作用
量子力学
认识论
物理
哲学
作者
Katarzyna A. Maltby,Krishna Sharma,Marc A. S. Short,Sannia Farooque,Rosalie Hamill,A. John Blacker,Nikil Kapur,Charlotte E. Willans,Bao N. Nguyen
出处
期刊:ACS Sustainable Chemistry & Engineering
[American Chemical Society]
日期:2023-05-30
卷期号:11 (23): 8675-8684
标识
DOI:10.1021/acssuschemeng.3c02164
摘要
Water-accelerated reactions, wherein at least one organic reactant is not soluble in water, are an important class of organic reactions, with a potentially pivotal impact on sustainability of chemical manufacturing processes. However, mechanistic understanding of the factors controlling the acceleration effect has been limited, due to the complex and varied physical and chemical nature of these processes. In this study, a theoretical framework has been established to calculate the rate acceleration of known water-accelerated reactions, giving computational estimations of the change to ΔG‡ which correlate with experimental data. In-depth study of a Henry reaction between N-methylisatin and nitromethane using our framework led to rationalization of the reaction kinetics, its lack of dependence on mixing, kinetic isotope effect, and different salt effects with NaCl and Na2SO4. Based on these findings, a multiphase flow process which includes continuous phase separation and recycling of the aqueous phase was developed, and its superior green metrics (PMI-reaction = 4 and STY = 0.64 kg L-1 h-1) were demonstrated. These findings form the essential basis for further in silico discovery and development of water-accelerated reactions for sustainable manufacturing.
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